Dielectric Barrier Discharge (DBD) Plasma Coating of Sulfur for Mitigation of Capacity Fade in Lithium–Sulfur Batteries

Sulfur particles with a conductive polymer coating of poly(3,4-ethylene dioxythiophene) “PEDOT” were prepared by dielectric barrier discharge (DBD) plasma technology under atmospheric conditions (low temperature, ambient pressure). We report a solvent-free, low-cost, low-energy-consumption, safe, and low-risk process to make the material development and production compatible for sustainable technologies. Different coating protocols were developed to produce PEDOT-coated sulfur powders with electrical conductivity in the range of 10–8–10–5 S/cm. The raw sulfur powder (used as the reference) and (low-, optimum-, high-) PEDOT-coated sulfur powders were used to assemble lithium–sulfur (Li–S) cells with a high sulfur loading of ∼4.5 mg/cm2. Long-term galvanostatic cycling at C/10 for 100 cycles showed that the capacity fade was mitigated by ∼30% for the cells containing the optimum-PEDOT-coated sulfur in comparison to the reference Li–S cells with raw sulfur. Rate capability, cyclic voltammetry, and electrochemical impedance analyzes confirmed the improved behavior of the PEDOT-coated sulfur as an active material for lithium–sulfur batteries. The Li–S cells containing optimum-PEDOT-coated sulfur showed the highest reproducibility of their electrochemical properties. A wide variety of bulk and surface characterization methods including conductivity analysis, X-ray diffraction (XRD), scanning electron microscopy (SEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and NMR spectroscopy were used to explain the chemical features and the superior behavior of Li–S cells using the optimum-PEDOT-coated sulfur material. Moreover, postmortem [SEM and Brunauer–Emmett–Teller (BET)] analyzes of uncoated and coated samples allowed us to exclude any significant effect at the electrode scale even after 70 cycles.